氢键介入的超分子亚胺离子催化研究

目前，不对称有机催化研究遇到的最大挑战是反应时间长、催化剂用量大，有些反应活性低等；另外一个重要的问题是寻找控制手性的新途径。亚胺离子催化是不对称有机催化领域重要的基本活化模式之一,为了解决该领域存在的这些难题，我们提出了"氢键介入的超分子亚胺离子催化"的概念。初步的研究发现，这一概念的使用不仅可以显著地提高反应时催化剂的活性，而且检测到了高浓度的亚胺离子的形成。因此，拟申请的此项目希望系统、深入地研究该概念，主要在以下方面展开：（1）超分子亚胺离子催化的新方法和新反应的设计和应用，希望用传统方法无法实现的一些反应可以在新的催化方法下有效地进行；(2)通过调控将产生多种多样的手性催化剂，在一些情况下可以避免或减少使用多步合成的复杂催化剂。（3）对超分子亚胺离子控制手性的方法进行深入研究。这些结果相信会成为传统方法的重要补充。

At present, the research in the field of asymmetric organocatalysis has been hampered by several limitations, such as long reaction time, high catalyst loading, low reactivity and so on. Another important topic is how to discover new approaches for stereocontrol. To this end, we designed and developed a new concept termed as "Hydrogen-Bond-Mediated Supramolecular Iminium Catalysis" for solving these long-standing challenge problems in iminium catalysis. We find this concept could be applied to solve these problems in iminium catalysis. Therefore, we would like to further develop this concept in this project. The proposal will focus on the following topics: 1) the design and application of new methods and new reactions in Supramolecular Iminium Catalysis that enables some inefficient reactions become work; 2)the stereocontrolling ability of the modularly designed supramolecular iminium catalysts will be powerful since they can be easily fine-tuned by simple modification or replacement of any of the components; as a consequence, a library of diverse catalysts could be used to make a wide range of supramolecular iminium catalysts enantioselective, while special tailored complex catalysts are avoided. 3）The study of new approaches of stereocontrol will be important challenge and significant application. These results will make important complementation to the limitations associated with traditional methods.